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Chinese Physics Letters

Controlling Population Transfer and Dissociation Rate of Na 2 Molecules with Ultra-Short Intense Laser Pulses

Kai‐Jun Yuan, Senming Wang, Shu‐Lin Cong

Published Sep 22, 2005• 8 citations
Publisher

Abstract

A scheme used for controlling the population transfer and the dissociation rate of Na 2 molecules is described by using the quantum wavepacket dynamical method. It is theoretically shown that the population transfer and the dissociation rate of Na 2 molecules can be controlled by pump and probe laser pulses with appropriate widths of pulses, sequence and intensities.

DOI
10.1088/0256-307x/22/10/021

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A scheme used for controlling the population transfer and the dissociation rate of Na 2 molecules is described by using the quantum wavepacket dynamical method. It is theoretically shown that the population transfer and the dissociation rate of Na 2 molecules can be controlled by pump and probe laser pulses with appropriate widths of pulses, sequence and intensities.
Abstract We theoretically investigate the complete population transfer among quantum states of the N a 2 molecule using ultrashort pulse trains using the time-dependent wave packet method. The population accumulation of the target state can be steered by controlling the laser parameters, such as the variable pulse pairs, the different pulse widths, the time delays and the repetition period between two contiguous pulses; in particular, the pulse pairs and the pulse widths have a great effect on the population transfer. The calculations show that the ultrashort pulse train is a feasible solution, which can steer the population transfer from the initial state to the target state efficiently with lower peak intensities.
Selective population transfer in electronic states of dissociative molecular systems is illustrated by adopting a control scheme based on Stark-chirped rapid adiabatic passage (SCRAP). In contrast to the discrete N-level system, dynamical Stark shift is induced in a more complex manner in the molecular electronic states. Wavepacket dynamics on the light-induced potentials, which are determined by the detuning of the pump pulse, can be controlled by additional Stark pulse in the SCRAP scheme. Complete population transfer can be achieved by either lowering the energy barrier along the adiabatic passage or placing the initial wavepacket on a well-defined dressed state suitable for the control. The determination of the pulse sequence is sufficient for controlling population transfer to the target state.
We demonstrate the feasibility of a laser induced complete population transfer to and from a continuum of states. We study the two-photon dissociation of v = 28; J = 1,...,10 sodium dimers. We demonstrate that using just a pair of "counter intuitively" ordered pulses we can dissociate 100% of the molecules in an ensemble. The scheme is shown to be stable with respect to the initial choice of rotational level and to fluctuations in the laser frequency and intensity. We also study the reverse phenomenon of complete population transfer from the continuum. We perform calculations on the radiative association of Na atoms to form the Na2 molecule in specific vib-rotational states. It is shown that two pulses of 20 nsec duration and as little as 6 MW/cm 2 peak power can photo-associate more than 98% of the atoms within a (pulse and velocity determined) relative effective distance, to yield Na2 molecules in the chosen v = 28; J = 10 vib-rotational state. This means that given a density of 10 16 atoms/cm 3 and a temperature of 7K, a 10Hz pulsed laser source of the above parameters can con- vert half of all the Na atoms in the ensemble to v = 28; J = 10 Na2 molecules within 15 seconds of operation.
Abstract By utilizing the time-dependent wavepacket method, we studied the population transfer between the electronic states of the Na 2 molecule driven by femtosecond laser pulses. Three electronic states, X 1 Σ g + , A 1 Σ u + and 2 1 Π g , are taken to be the initial, the intermediate and the target states, respectively. Two classes of calculations are performed for comparison: one is to invoke the rotating wave approximation (RWA), and the other is more accurate calculations without consideration of RWA (non-RWA). It is found that for this three-state-model, the RWA fails to describe the accurate population transfer process in femtosecond-pulse fields and that the adiabatic passage is hard to be constructed in the non-RWA calculations. Based on the non-RWA calculations, we determined a set of laser parameters, including the peak intensity, detuning, pulse duration and time delay, for efficient population transfer.
Laser control of complete vibrational transfer in Na2_22​ using resonance coalescence
With a specific choice of laser parameters resulting into a so-called exceptional point in the wavelength-intensity plane, it is possible to produce the coalescence of two Floquet resonances describing the photodissociation of the molecule Na2_22​, which is one of the candidates for molecular cooling. Appropriately tuning laser parameters, following a contour around the exceptional point, the resonances exchange their labels. This represents a laser control of the vibrational transfer from one field-free state to another, through an adiabatic transport involving these resonances. The proportion of undissociated molecules at the end of the pulse is checked through Floquet adiabatic theory. A vibrational cooling scenario can be proposed based on a complete vibrational transfer which is predicted, with only 20 percent of molecules undergoing dissociation.